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Metal nanoclusters have a certain rigidity due to their specific coordination patterns and shapes; thus, they face extreme difficulty in folding into a specific direction to form a double‐helix structure and in further interconnecting to form metal–helix frameworks (MHFs). To date, no MHFs have been produced by the formation of heterometallic clusters. Selecting the appropriate "bonding molecules" to bond metal nanoclusters in a specific multiple direction is one of the most effective strategies for designing synthetic MHFs. In this study, we realized for the first time the control of different orientations of μ3‐NO3− to join heterometallic clusters (Cu10Dy2) and subsequently form a left‐handed double helix chain, which further joins to form MHFs. In the structure of the MHFs, four different directions of bridging μ3‐NO3− exist, three of which are involved in the linkage of the double‐helix chain. Each μ3‐NO3− is connected to three adjacent Cu10Dy2. Herein, we extend a new method for designing synthetic double‐helix structures and MHFs, thereby further laying the foundation for the development of similar DNA double‐helix structures and nucleic acid secondary structures in vitro. [ABSTRACT FROM AUTHOR]